Interesting question! Everyone plays different I guess, but I think the 'no happy environment' mod is a big one. TS4 has a good mood system but it ends up being totally overwhelmed by happy moodlets for the environment. It's not that I don't like this moodlet, but it's overpowered and happens too often and too much on typical lots with lots of decorative items. When it's taken out the mood system suddenly gets a lot more realistic and interesting.
Agree with everyone else who said MCCC, it just gives lots of important options to make the world work how you want it to.
I found the money system didn't work great for me, it seems too easy to get rich. I use MCCC to set bills higher. I also use mods to increase the cost of university fees. However, I also use a mod that makes the pay higher as sims go up the career scale. I feel that's more realistic as sims with higher careers get wealthy, and keeps the lifestyle of sims with less income more realistic. I don't expect my sims who own a pineapple farm to become really wealthy as time goes by! The income from growing/crafting things seemed overpowered to me so this helps a lot. It also makes fancy houses authentically expensive to live in.
The gallery is great too. I have issues with navigating it, but for content there's loads of great builds and sims to download when you start finding creators you like. I often edit the sims or remodel builds off there, I use it a lot to add interesting sims and builds to the world.
For gameplay mods I like simsonian library. The freelance entertainer, archeaology, and family history mods add loads of gameplay.
For DLC that makes the world more interesting, seasons is a big one for me, it makes all the worlds more dynamic and the changing seasons and calendar activities keep things interesting. It isn't like the same day over and over again.
I think EPs and game packs give a lot more for your money per € than stuff packs and kits. I do enjoy bowling night and castle estates though, I've gotten quite a lot out of those - but I like bowling and I like castles! It's a bit specific to you I think. But if you're on a budget, I'd definately lean towards EPs and game packs before anything else. They give more objects, gameplay and worlds to build in.